Comb potential - Cuprous oxide

[Andreas_Ruhl]

Hi,

I wanted to test the Comb potential by simulating a simple bulk structure of cuprous oxide. Unfortunately the structure isn't stable in the simulation. I attached my input file and the restart file for the bulk configuration, because I don't know where the problem might be. I'm pretty sure that the configuration file for cuprous oxide is correct (It's based on a cubic cell with a lattice parameter of 4.27 A), although it looks like I started with an off equilibrium configuration.
Be that as it may, the problem is, that I'm not familiar with the comb potential, especially the charge equilibration is totally new to me. So maybe the error is located in a wrong setting and therefore it would be nice if the comb experts can take a loot at my input file for crucial mistakes. I should add, that wether or not defining new start values of the charges, the result keeps the same. The structure isn't stable and the temperature rises up to ca. 4000 K.
Best regards,
Andreas Rühl

#------------- inputfile ---------------------------
  ---------- Initialize Simulation

[Ray_Shan]

Hi,

I wanted to test the Comb potential by simulating a simple bulk
structure of cuprous oxide. Unfortunately the structure isn't stable in
the simulation. I attached my input file and the restart file for the
bulk configuration, because I don't know where the problem might be. I'm
pretty sure that the configuration file for cuprous oxide is correct
(It's based on a cubic cell with a lattice parameter of 4.27 A),
although it looks like I started with an off equilibrium configuration.
Be that as it may, the problem is, that I'm not familiar with the comb
potential, especially the charge equilibration is totally new to me. So
maybe the error is located in a wrong setting and therefore it would be
nice if the comb experts can take a loot at my input file for crucial
mistakes. I should add, that wether or not defining new start values of
the charges, the result keeps the same. The structure isn't stable and
the temperature rises up to ca. 4000 K.
Best regards,
Andreas Rühl

#------------- inputfile ---------------------------
  ---------- Initialize Simulation
---------------------------------------------

clear
units metal
dimension 3
boundary p p p
newton on

#internal storage of atom attributes
atom_style charge
atom_modify map array

# ---------- Create Atoms
------------------------------------------------------

variable nsteps equal 2000

read_data CuO_750_bulk

# ---------- Define Interatomic Potential
--------------------------------------
mass 1 63.546
mass 2 15.9994
set type 1 charge 0.008
set type 2 charge -1.41

The system is not charge neutral with these set commands, which is the
cause of the instability.

pair_style comb
pair_coeff * * ffield.comb Cu O

# ---------- Define Settings
---------------------------------------------------
#neighbor list settings
neighbor 2.0 bin
neigh_modify delay 10 check yes

#assigning starting velocities
#velocity all create 300.0 4128459 mom yes dist gaussian

# ---------- Run Minimization ---------------------
reset_timestep 0 #if timestep isn't 0

#operation on particles
fix c_equ all qeq/comb 10 0.00001 file charge_output

A precision/tolerance of 1e-5 is too small - 1e-3 is usually better.

Ray

[Andreas_Ruhl]

Hi,

thanks Ray for the quick reply. Of course, the charge neutrality should be guaranteed. So I deleted the set charge commands and also used a new configuration file, because the charges didn't sum up to zero either. Unfortunately it is still not working as expected. The temperature rises up to 4000 K, starting from zero K.

Did I do something else wrong in the set up? If not, the mistake must be in the configuration file (Like I told before, it should be alright. If one just looks at the first 6 atoms, you find the unit cell of my bulk configuration, which should be one possible unit cell of cuprous oxide).
I attached the new configuration file. The set up is basically the same as before, without the set charge commands and the precision of charge equilibration set to 10e-3 . Maybe someone can reproduce this behaviour.
Help would be really appreciated.
Best regards,
Andreas Rühl

LAMMPS data file via write_data, version 1 Feb 2014, timestep = 0

750 atoms
2 atom types

0.0000000000000000e+00 2.1349999999999998e+01 xlo xhi
0.0000000000000000e+00 2.1349999999999998e+01 ylo yhi
0.0000000000000000e+00 2.1349999999999998e+01 zlo zhi

Masses

1 63.546
2 15.9994

Atoms

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[Ray_Shan]

If you are certain the structure is correct and the charges sum to zero, you might want to start with minimization.

Ray

[Ray_Shan]

One more thing. When you see temperature spikes using any kind of potentials, what would be the natural thing to do? Decrease timestep size.

Ray

[Andreas_Ruhl]

I thought minimization (fix box/relax) wasn't possible with the comb potential, because of the charge equilibration. At least I read something like this in the mailing archive. Or what do you mean with minimization.

Andreas

[Ray_Shan]

Mailing list archive is old and the fix qeq/comb doc page is up to date. Yes, you can use qeq with minimization.

Ray

[Andreas_Ruhl]

So I did a minimization and in the process of that, I found out a few new things.

First the result of the minimization was a small shrinking of the box. Now the lattice constant was something like a=4.17 instead of a=4.27. Which is strange, because the potential should reproduce the lattice constant according to the published paper. Even more confusing, the now relaxed structure remained stable in a simulation.

But I also observed a strange cooling of the structure in that simulation. So when I took a closer look, I saw that the totally energy wasn't conserved in the nve simulation. There was something like an exponential decrease in the total energy. So I took a step back and looked at the results of my previous failing simulations with the unrelaxed structure. And there was also a loss in total energy observable. I hadn't seen it the first time, because I just focused on the rapidly increasing temperature.

So in summary, this loss in energy seems to be the main problem. Which has to be the potential and a possible wrong set up of it. If the structure isn't the ideal structure, then, at least, the total energy stays constant or shouldn't it? I also tried a smaller timestep. It has no improving effect.
Any explanation for this?

Andreas

[Ray_Shan]

It could be bad fix qeq/comb settings, bad charge convergence, bad setup, bad structure, etc. Without full input deck, nobody knows.

[Andreas_Ruhl]

I attached the requested input deg.
In the meantime I found out that the energy loss has something to do with the charge convergence, because if you look closely, one sees that the energy is dropping in steps, exactly every time a charge equilibration is performed. In my case every tenth time step.
Hope you can work with this and also thanks for your effort so far.
Andreas

ffield.comb (19.2 KB)

in.muster (1.26 KB)

start_config (130 KB)

[Ray_Shan]

My suggestion of reducing the time step was apparently not taken…… Why don’t you try with 0.1 fs?

Mind you, QEq using damped dynamics solver (Rick JCP 101, 6141 (1994)) does not conserve energy due to damping (see Yu PRB 75, 085311 (2007)). So you will always see a drift in total energy with fix qeq/comb.

Ray

[Andreas_Ruhl]

Believe me, I did also a simulation with 0.1fs. I simply changed it back to 1fs in the input file. For the smaller timestep the drift was just not so big.

But now that I know, that the drift is an intrinsic effect of charge equilibration, let me then come back to original problem:
CuO bulk with a=4.27 not stable, after minimization CuO bulk with a=4.17 stable. Isn't the a=4.17 wrong? I find that confusing. That's why, I attached the input deck for the original bulk structure with (!) timestep 0.1 fs and a=4.27.

And just to be on the safe side, the structure is based on the following unit cell:
cubic cell, a1=(a,0,0) a2=(0,a,0) a3=(0,0,a) with a=4.27
atom positions: Cu (0,0,0) (0,0.5,0.5) (0.5,0.5,0) (0.5,0,0.5)
                             O (0.25,0.25,0.25) (0.75,0.75,0.75)

If this is the correct unit cell for CuO bulk, the simulation with the provided input deck should be stable. But when I run it, it isn't. Also with a timestep of 0.1 fs, and even 0.01 fs.
I would be very thankful, if you can try to reproduce it (I know you, you have better things to do). At least, then I can exlude, that for example the executable was somehow wrongly compiled.

Andreas

CuO_750_bulk (131 KB)

ffield.comb (19.2 KB)

in.muster (1.26 KB)

[Ray_Shan]

I get a=4.265 with the attached input files.

Ray

[Ray_Shan]

in.comb (1.06 KB)

ffield.comb (19 KB)

[Andreas_Ruhl]

Thank you very much for the attached files, because with these I found out that you have a different ffield.comb file. I ran first your input script with your potential file and got the same result. But when I used my potential file I got again the smaller lattice constant a=4.17.
I looked into both files, and indeed, some parameters are just different. To be sure that I have the right potential file I checked the ffield.comb in the current Lammps branch and it was the same. So somehow you have a different ffield.comb than provided in the Lammps potential folder.

One additional remark. Have you tried to do a longer simulation with your input deck. When I take your input deck, go to higher temperature (3K is enough) and do a simulation run after the minimization with, let's say, 2000 steps, the temperature increases at some point rapidly. Does this happen for you too?

Andreas